连续性气相催化转化低浓度生物燃气制甲醇

陆志恒; 谢玄兰; 李文志

doi:10.19912/j.0254-0096.tynxb.2025-0142

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太阳能学报 ›› 2026, Vol. 47 ›› Issue (4) : 467-477. DOI: 10.19912/j.0254-0096.tynxb.2025-0142

连续性气相催化转化低浓度生物燃气制甲醇

陆志恒¹, 谢玄兰¹, 李文志²

作者信息 +

CONTINUOUS GAS PHASE CATALYTIC CONVERSION OF LOW CONCENTRATION BIOGAS TO METHANOL

Lu Zhiheng¹, Xie Xuanlan¹, Li Wenzhi²

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文章历史 +

摘要

采用浸渍法制备一系列铜基沸石催化剂（xCu/MOR）,并在以水为氧化剂的连续性气相条件下开展催化生物燃气部分氧化制甲醇性能研究。结果表明,350 ℃条件下,甲醇产率随着铜负载量的增加呈火山型趋势,其中2Cu/MOR催化剂可实现67.3 μmol/（g·h）的高甲醇产率;进一步优化反应温度,2Cu/MOR催化剂在400 ℃反应条件下甲醇产率高达142.5 μmol/（g·h）。此外,使用X射线衍射、高分辨透射电子显微镜、X射线光电子能谱、紫外-漫反射可见光谱、甲烷程序升温脱附及傅里叶变换红外光谱技术进行催化剂表征分析,结果表明铜基沸石催化剂中铜元素分散均匀,表现出优异活性的2Cu/MOR催化剂有更多的孤立二价铜活性位点,反应过程中甲烷在孤立二价铜位点上吸附活化,形成的甲氧基中间体与水解离产生的羟基反应生成甲醇。

Abstract

A series of copper-based zeolite catalysts （xCu/MOR） were prepared by impregnation method, and the performance of catalytic partial oxidation of biogas to methanol was investigated under continuous gas-phase conditions with water as oxidant. The results show that the methanol yield at 350 ℃ shows a volcano trend with the increase of copper loading, in which the 2Cu/MOR catalyst can achieve a high methanol yield of 67.3 μmol/（g·h）; further optimization of the reaction temperature results in a high methanol yield of up to 142.5 μmol/（g·h） for the 2Cu/MOR catalyst at 400 ℃. In addition, catalyst characterization using X-ray diffraction, high-resolution transmission electron microscopy, X-ray photoelectron spectroscopy, UV-diffuse reflectance visible spectroscopy, methane programmed warming desorption, and Fourier transform infrared spectroscopy show that the copper element in the copper-based zeolite catalysts is uniformly dispersed, and the 2Cu/MOR catalysts that demonstrated excellent activity have more isolated divalent copper active species. During the reaction process, methane is adsorbed and activated on the isolated divalent copper sites, and the formed methoxy intermediate reactes with the hydroxyl group produced by hydrolysis to form methanol.

导出引用

陆志恒, 谢玄兰, 李文志. 连续性气相催化转化低浓度生物燃气制甲醇[J]. 太阳能学报. 2026, 47(4): 467-477 https://doi.org/10.19912/j.0254-0096.tynxb.2025-0142

Lu Zhiheng, Xie Xuanlan, Li Wenzhi. CONTINUOUS GAS PHASE CATALYTIC CONVERSION OF LOW CONCENTRATION BIOGAS TO METHANOL[J]. Acta Energiae Solaris Sinica. 2026, 47(4): 467-477 https://doi.org/10.19912/j.0254-0096.tynxb.2025-0142

中图分类号： TQ223

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